production combination is ethanol (low value) and succinic acid (high value), together with acetic acid and electricity as co-products.

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1 Summary The increasing world energy demand, depletion and unequal distribution of fossil resources, and the dangers caused by climate change are the driving forces for the development of alternative energy sources. In view of the GHG emission reduction target agreed upon in the Kyoto protocol, a shift from fossil fuels to renewable resources is ongoing to secure the long-term energy supply at both national and international level. Renewable energy is generated from natural resources such as sunlight, wind, waves and geothermal heat. In 2006, about 18% of global energy consumption came from renewables, 13% of which was from traditional biomass such as wood combustion. Hydroelectricity was the second largest renewable source, providing 3% of global energy consumption. To keep up with the growing energy demand, many nations have established new regimes on renewable energy. For instance, the European Commission decided in 2007 on a 20% target for the overall share of energy from renewable sources and a 10% target for energy from renewable sources in transport by At least for the foreseeable future, low-carbon fuels in liquid form are required for use in existing internal combustion engines in transportation. Biofuels are potential lowcarbon energy sources, and can provide energy for the transport sector. With the available conversion technologies they may contribute substantially to achieving the renewable energy targets in the near future. Biomass, with its abundance and renewable nature, is available as a feedstock for the production of fuels. Examples of biomass that can be used to produce fuels include conventional crops (corn, wheat, rice, sorghum, sugarcane, sugar beet, cassava, palm oil, rapeseed, etc.), agricultural residues (corn stover, wheat and rice straw, sugarcane bagasse etc.) and dedicated cellulosic plants (poplar, switchgrass and miscanthus, for example). Against the background of the ongoing debate on biofuels and biorefining, the objective of this thesis is to indicate possible directions for biomass refining for sustainable development, focusing on environmental and economic analyses of the refining of lignocellulosic biomass. To this end, three main research questions have been formulated: 149

2 I. Is fuel ethanol from lignocelluloses better than gasoline, from an environmental point of view? II. How can bio-based production be optimized with regard to energy efficiency, environmental performance and economic feasibility? III. How can we design a methodology to achieve a more comprehensive sustainability assessment of biomass refining? With regard to the first question, life cycle assessment (LCA) was chosen as an analysis tool, as it is capable of handling fuel systems on a life cycle basis. Three chapters of this thesis are dedicated to comparative life cycle assessment (LCA), with different focuses: Chapter 2 addresses one of the most important methodological issues in LCA allocation, using fuel ethanol from corn stover as a case study. It concludes that the comparison of fossil fuels with biofuels is highly sensitive to the choice of allocation method. Chapter 3 compares the environmental performance and cost of fuel ethanol for two scenarios in Brazil: current practice ethanol and sugar production from juice sugar, and electricity co-generation from combustion of bagasse and the future case, in which ethanol and sugar are produced from juice sugar and bagasse is also used to produce ethanol, while electricity is generated from the combustion of lignin residues and wastes. It is concluded that the system using bagasse to produce electricity has a better environmental performance than the system in which ethanol is produced from it. Chapter 4 focuses on LCA for another promising feedstock, switchgrass, and analyzes the changes in environmental impact relating to the choice of allocation, soil preparation and transport distance. Compared to the stover- and sugarcane-ethanol systems, this is a relatively simpler chain, because switchgrass is a dedicated energy crop for ethanol production, without agricultural co-products. Moreover, only a small amount of surplus electricity is co-generated in the ethanol production process, which makes the choice of allocation easier no allocation is needed in agricultural production. Switchgrassethanol seems to have a much better environmental performance than gasoline. In order to compare and evaluate the environmental performance of bioethanol from lignocelluloses with that of gasoline, Chapter 6 summarizes the results reported in Chapters 2, 3 and 4, and two more studies on ethanol production from flax shives and hemp hurds. In all these studies, the same technologies were used to convert cellulose and hemicellulose to ethanol and to generate heat and power from lignin and wastes; the same system boundaries were defined; and the same allocation procedures were 150

3 followed. A comprehensive set of environmental impacts is addressed, ranging from abiotic resource depletion and GHG emissions to acidification, eutrophication and toxicity aspects. The findings from these four chapters present a clear example of problem shifting solving the problems of oil depletion and ozone depletion at the expense of increasing agriculture-related emissions, which contribute significantly to eutrophication and toxicity aspects, as well as to global warming via N2O emissions. Moreover, the outcomes of LCA especially in terms of global warming greatly depend on the choice of allocation method. If agricultural co-products are utilized for ethanol production, the GHG performance greatly depends on the amount of carbon dioxide uptake that is allocated to the lignocellulosic co-products. These two issues make it difficult to conclude whether, from an environmental point of view, fuel ethanol from lignocelluloses is better than gasoline. However, bioethanol certainly has potential in terms of reducing fossil resource use, as well as in GHG emissions, if more promising feedstocks like switchgrass and sugarcane are used. The limitations lie in the agricultural production of biomass. Savings can be offset by poor management, for instance due to the loss of soil organic matter, or high emissions of nitrous oxide (N2O) if too much nitrogen fertilizer is used. Technology development, improved agricultural practice and reduction of land use are crucial to reducing the environmental impact. In relation to the second question, Chapter 5 presents a detailed energy analysis of the corn stover-based ethanol system, and the resulting energy inputs in sub-processes point out directions for process optimization in terms of energy efficiency. The estimated net energy values are compared with the literature values on first-generation bioethanol to assess more accurately whether second-generation ethanol is more energy efficient. Chapter 6 compares the net energy values obtained from Chapter 5 with those from selected literature studies on the same subject. These studies have mainly focused on corn-, stover-, switchgrass- and sugarcane-derived ethanol systems. Two types of accounting are used including and excluding co-products and energy credits. A single-product (ethanol) system can be optimized only to a certain extent, due to the fixed process options and relatively low price of ethanol. Full optimization in terms of energy efficiency, environment and economy should focus on an integrated production system multi-product biorefinery. Chapter 7 reports on the design of a lignocellulosic feedstock biorefinery producing fuel, chemicals and power in one plant, and analyzes the environmental and economic potential of such a refinery. In this case, the selected 151

4 production combination is ethanol (low value) and succinic acid (high value), together with acetic acid and electricity as co-products. The outcomes reported in Chapter 5 and Chapter 6 indicate that the energy-intensive processes in the ethanol life cycle are fertilizer production, tillage and harvesting in agriculture, and pre-treatment, product recovery and enzyme production in the ethanol production. These findings suggest options for optimization in terms of process technology and energy efficiency. Moreover, when the energy credits of all co-products are taken into account, ethanol production from cellulosic feedstocks is much more energy efficient than corn-based ethanol. With regard to environmental performance, improvements can be achieved by selecting feedstocks which require less intensive agricultural practices. Chapter 7 demonstrates that multi-product biorefining can indeed be more feasible technically, economically as well as environmentally than single-output productions such as an ethanol plant, especially when an appropriate product combination is chosen. Essential in the refinery design in this thesis is the fact that the CO2 generated is not emitted, but used in the process of succinic acid production. Although the refinery in this thesis was designed with highly optimized technology, further development and improvements could be made. However, we should keep in mind that optimization in terms of process technology and energy efficiency may bring side-effects not just poorer environmental performance, but also lower profitability or a lower acceptability to society. Regarding the last research question, this thesis starts with a methodology widely used in biofuel studies life cycle assessment. Chapter 2 investigates the influence of allocation methods on outcomes and indicates the limitations of LCA methodology. Three allocation methods are discussed mass/energy-based allocation, economic value-based allocation and system expansion. These are combined with a sensitivity analysis for the treatment of biogenic carbon: leaving biogenic carbon out of the analysis, as is usual in many biofuel studies, or accounting for both extractions and emissions of CO2, as is standard LCA practice. These issues appear to be essential in a biofuel-fossil fuel comparison. Chapter 3 involves life cycle costing (LCC) of the fuel ethanol system using a steady state cost model, in which only production costs are taken into account. This can give an indication of the economic feasibility but does not reflect the dynamic effect in the real market. The results of both LCA and LCC are compared with those of the gasoline system. 152

5 The results reported in these two chapters suggest that the development of methodologies beyond LCA is essential, especially for multi-product systems such as biorefineries. Chapter 7 assesses the economic feasibility of a newly designed biorefinery using economic modelling that reflects market effects. It further develops an ecoefficiency indicator (emissions per unit of value derived) to analyze the environmental impact of the refinery without applying an allocation procedure. Although the methodology developed for system analysis in this chapter is based on LCA, it is expanded beyond LCA. Although LCA is a tool developed for decision-making in sustainable development, it is innately prone to discrepancies, being heavily reliant on methodological choices and assumptions made. Chapter 2 concludes that LCA as it stands has a number of limitations. First of all, outcomes are greatly dependent on the allocation method applied; secondly, important impacts such as land and water use are not yet included in standard LCA databases; thirdly, issues related to indirect land use changes and competition with food products do not fit well into the LCA framework; and finally, LCA is also limited in terms of handling multi-output systems, such as complex biorefineries. The results of LCC on ethanol derived from sugarcane indicate that driving on ethanol fuels is more economical than on gasoline, and that the future case is economically more attractive than the base case, which has probably been the driving force for the promotion of advanced technologies converting bagasse to ethanol. Due to the steady-state cost model used in LCC, the results can only provide a preliminary indication of the economic feasibility of the process. In the real market, the prices of fuels are very much dependent on taxes and subsidies. The findings reported in these two chapters urge us to develop a broader approach to analyze the environmental performance and profitability of a multi-product biorefinery system. The eco-efficiency indicator used in Chapter 7 presents one example of such an approach, which is based on a cradle-to-gate LCA methodology. The difference between this approach and the methodology of LCA and LCC lies in accounting for the environmental impact of the whole system and the values derived from it. Since this avoids allocation, it is considered a methodology based on LCA but going beyond LCA. Sustainability has implied the integration of the economic, social and environmental spheres to meet the needs of the present generation without compromising the ability of future generations to meet theirs. This thesis has addressed the directions and perspectives of biomass refining, especially to produce fuels and chemicals, for sustainable development. Methodologies for this critical analysis and assessment have 153

6 been developed and applied. Although social aspects were beyond the scope of this study, they have been extensively discussed in some literature studies, including the dilemma fuel for the rich or food for the poor caused by the biofuels regime. Such concerns should be on the mind of every responsible leader in government, business and civil society. On a global scale, dialogues among nations help to better understand regional problems and needs. Exchanging information and sharing technologies create opportunities for the developing nations, whilst new initiatives create incentives for simultaneous local and global sustainable development. More importantly, these matters should be a concern for every citizen, because collective sustainability is also an individual responsibility. 154